The relation between macro-properties and micro-quantities of the large-grained polycrystalline chemical vapour deposited diamond films was investigated. Considering the growth non-uniformity, the micro-Raman spectra measured on the top growth surface show large variation from spot to spot. Whereas, the micro-Raman spectra taken on the fine-grained smooth interface of the diamond films show that small deviation and generally can represent the overall quality of the large-grained polycrystaline diamond films, and correlate well with hydrogen content of the film measured by Fourier-transform infrared spectroscopy. It can be concluded that a diamond film with darker color or lower transparency has lower quality and lower phase purity characterized by the larger full width at half maximum (FWHM) and lower intensity of the diamond Raman peak around 1 332 cm－1.